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Visualizing interfacial collective reaction behaviour of Li–S batteries

Author

Listed:
  • Shiyuan Zhou

    (Xiamen University)

  • Jie Shi

    (Beijing University of Chemical Technology)

  • Sangui Liu

    (Xiamen University)

  • Gen Li

    (Xiamen University)

  • Fei Pei

    (Xiamen University)

  • Youhu Chen

    (Xiamen University)

  • Junxian Deng

    (Xiamen University)

  • Qizheng Zheng

    (Xiamen University)

  • Jiayi Li

    (Nanjing University)

  • Chen Zhao

    (Argonne National Laboratory)

  • Inhui Hwang

    (Argonne National Laboratory)

  • Cheng-Jun Sun

    (Argonne National Laboratory)

  • Yuzi Liu

    (Argonne National Laboratory)

  • Yu Deng

    (Nanjing University)

  • Ling Huang

    (Xiamen University)

  • Yu Qiao

    (Xiamen University
    Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM))

  • Gui-Liang Xu

    (Argonne National Laboratory)

  • Jian-Feng Chen

    (Beijing University of Chemical Technology)

  • Khalil Amine

    (Argonne National Laboratory)

  • Shi-Gang Sun

    (Xiamen University)

  • Hong-Gang Liao

    (Xiamen University
    Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM))

Abstract

Benefiting from high energy density (2,600 Wh kg−1) and low cost, lithium–sulfur (Li–S) batteries are considered promising candidates for advanced energy-storage systems1–4. Despite tremendous efforts in suppressing the long-standing shuttle effect of lithium polysulfides5–7, understanding of the interfacial reactions of lithium polysulfides at the nanoscale remains elusive. This is mainly because of the limitations of in situ characterization tools in tracing the liquid–solid conversion of unstable lithium polysulfides at high temporal–spatial resolution8–10. There is an urgent need to understand the coupled phenomena inside Li–S batteries, specifically, the dynamic distribution, aggregation, deposition and dissolution of lithium polysulfides. Here, by using in situ liquid-cell electrochemical transmission electron microscopy, we directly visualized the transformation of lithium polysulfides over electrode surfaces at the atomic scale. Notably, an unexpected gathering-induced collective charge transfer of lithium polysulfides was captured on the nanocluster active-centre-immobilized surface. It further induced an instantaneous deposition of nonequilibrium Li2S nanocrystals from the dense liquid phase of lithium polysulfides. Without mediation of active centres, the reactions followed a classical single-molecule pathway, lithium polysulfides transforming into Li2S2 and Li2S step by step. Molecular dynamics simulations indicated that the long-range electrostatic interaction between active centres and lithium polysulfides promoted the formation of a dense phase consisting of Li+ and Sn2− (2

Suggested Citation

  • Shiyuan Zhou & Jie Shi & Sangui Liu & Gen Li & Fei Pei & Youhu Chen & Junxian Deng & Qizheng Zheng & Jiayi Li & Chen Zhao & Inhui Hwang & Cheng-Jun Sun & Yuzi Liu & Yu Deng & Ling Huang & Yu Qiao & Gu, 2023. "Visualizing interfacial collective reaction behaviour of Li–S batteries," Nature, Nature, vol. 621(7977), pages 75-81, September.
  • Handle: RePEc:nat:nature:v:621:y:2023:i:7977:d:10.1038_s41586-023-06326-8
    DOI: 10.1038/s41586-023-06326-8
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    Citations

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    Cited by:

    1. Zhiyuan Han & An Chen & Zejian Li & Mengtian Zhang & Zhilong Wang & Lixue Yang & Runhua Gao & Yeyang Jia & Guanjun Ji & Zhoujie Lao & Xiao Xiao & Kehao Tao & Jing Gao & Wei Lv & Tianshuai Wang & Jinji, 2024. "Machine learning-based design of electrocatalytic materials towards high-energy lithium||sulfur batteries development," Nature Communications, Nature, vol. 15(1), pages 1-13, December.
    2. Xiongwei Zhong & Xiao Xiao & Qizhen Li & Mengtian Zhang & Zhitong Li & Leyi Gao & Biao Chen & Zhiyang Zheng & Qingjin Fu & Xingzhu Wang & Guangmin Zhou & Baomin Xu, 2024. "Understanding the active site in chameleon-like bifunctional catalyst for practical rechargeable zinc-air batteries," Nature Communications, Nature, vol. 15(1), pages 1-17, December.
    3. Zhen Wu & Mingliang Liu & Wenfeng He & Tong Guo & Wei Tong & Erjun Kan & Xiaoping Ouyang & Fen Qiao & Junfeng Wang & Xueliang Sun & Xin Wang & Junwu Zhu & Ali Coskun & Yongsheng Fu, 2024. "Unveiling the autocatalytic growth of Li2S crystals at the solid-liquid interface in lithium-sulfur batteries," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    4. Qin Yang & Jinyan Cai & Guanwu Li & Runhua Gao & Zhiyuan Han & Jingjing Han & Dong Liu & Lixian Song & Zixiong Shi & Dong Wang & Gongming Wang & Weitao Zheng & Guangmin Zhou & Yingze Song, 2024. "Chlorine bridge bond-enabled binuclear copper complex for electrocatalyzing lithium–sulfur reactions," Nature Communications, Nature, vol. 15(1), pages 1-13, December.
    5. Ji Hwan Kim & Mihyun Kim & Seong-Jun Kim & Shin-Yeong Kim & Seungho Yu & Wonchan Hwang & Eunji Kwon & Jae-Hong Lim & So Hee Kim & Yung-Eun Sung & Seung-Ho Yu, 2024. "Understanding the electrochemical processes of SeS2 positive electrodes for developing high-performance non-aqueous lithium sulfur batteries," Nature Communications, Nature, vol. 15(1), pages 1-13, December.

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